Traceability and dispersion of highly toxic soluble phases from historical mine tailings

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Limited research has been done on traceability from historical mining sites in arid and semi-arid regions. Pb isotope systematics was applied to decipher the importance of identifying the mixing of lead sources involved in forming efflorescent salts and the repercussions on traceability. This research assessed mine waste (sulfide-rich and oxide-rich tailings material and efflorescent salts) and street dust from surrounding settlements at a historical mining site in northwestern Mexico, focusing on Pb isotope composition. The isotope data of tailings materials defined a trending line (R 2 = 0.9); the sulfide-rich tailings materials and respective efflorescent salts yielded less radiogenic Pb composition, whereas the oxide-rich tailings and respective efflorescent salts yielded relatively more radiogenic compositions, similar to the geogenic component. The isotope composition of street dust suggests the dispersion of tailings materials into the surroundings. This investigation found that the variability of Pb isotope composition in tailings materials because of the geochemical heterogeneity, ranging from less radiogenic to more radiogenic, can add complexity during environmental assessments because the composition of oxidized materials and efflorescent salts can mask the geogenic component, potentially underestimating the influence on the environmental media. Historical mine tailings Pb isotopes PTE dispersion traceability efflorescence salts Figures Figure 1 Figure 2 Figure 3 Figure 4 1. Introduction Efflorescence salts are naturally occurring secondary minerals in various environments, including mine waste. In the context of mine waste, the efflorescent salts can accumulate and momentarily immobilize metals, which can be released later in solution, as they commonly consist of highly soluble phases (Lottermoser, 2017 ). Additionally, efflorescent salts are characterized by low cohesion and density, facilitating decrepitation, lifting, and wind dispersion (Del Rio-Salas et al., 2019 ; Punia, 2021). Therefore, although ephemeral, they are quite effective in dispersing potential toxic elements (PTE) into the environment. Among the different types of mine waste (mining, mineral processing, metallurgical, etc.), mine tailings impoundments are considered the largest and most dangerous industrial infrastructures worldwide (Davies, 2002 ). Mine tailings are constructed to confine the waste during the mine’s operational life and after closure. They contain fine-grained materials, including minerals, rock fragments, sediments, chemical reactants, and water. Tailings impoundments generated during historical mining commonly contain higher PTE contents than those from active mines due to less efficient metallurgical processes and laxer environmental standards at the time, among other reasons (e.g., Del Rio-Salas et al., 2019 ). Particularly in developing countries, historical tailings impoundments lack containment, monitoring, and remediation programs and have become part of the landscape (e.g., Peña-Ortega et al., 2019 ). PTE content in historical mine tailings is related to metal commodities allocated within sulfide minerals after processing. Exposure to air and humidity triggers the breakdown of sulfides through oxidation processes, producing acidic waters enriched in sulfate and PTE, a phenomenon widely known as acid mine drainage (AMD) (Lottermoser, 2010 ; 2017 ). AMD is critical in arid and semi-arid environments since high temperatures, torrential rains, high evaporation rates, and capillarity action favor the migration of PTE-bearing fluids to the tailings surface, precipitating the efflorescent salts (Khorasanipour, 2015 ) composed mainly by sulfates, in addition to chlorides, nitrates, among other mineral species. Understanding the dispersion of tailings materials and efflorescent salts is essential not only because of their high capacity to contaminate different environmental media such as soil, water, and dust but also because of their high potential toxicity to humans (Gonzalez et al., 2014; Pérez-Sirvent et al., 2016 ; Loredo-Jasso et al., 2021 ; Martínez-López et al., 2021 ; Punia 2021). Specifically, efflorescent salts and relatively high PTE contents related to mine tailings have been identified in sediments (García-Lorenzo et al., 2012 ) and dust from rural settlements near historical mining sites (Del Rio-Salas et al., 2019 ). In the latter scenario, rural dust can serve as the final fate for PTE associated with mine tailings and efflorescent salts; detecting efflorescent salts and high PTE concentration in rural dust underscores their dispersal capacity despite their temporary nature. Among different techniques to assess dispersion, Pb isotope systematics has effectively traced Pb in various research fields, including petrogenesis, tectonics, ore deposits, anthropology, forensic sciences, environmental sciences, etc. Lead has four naturally occurring stable isotopes ( 204 Pb, 206 Pb, 207 Pb, and 208 Pb); 204 Pb is non-radiogenic, while 206 Pb, 207 Pb, and 208 Pb are the decay products of 238 U, 235 U, and 232 Th, respectively (Dickin, 1995 ). Lead does not fractionate, and particularly in environmental studies, processes such as emission, transport, and deposition do not affect the isotope composition, enabling source identification (geogenic vs. anthropogenic) and tracing dispersion of PTE in environmental media (e.g., dust, particulate matter, soils, sediments, plants, mine waste) and organisms (i.e., Dong et al., 2020 ; Fry et al., 2020 ; Lee et al., 2019 ; McPartland et al., 2020 ; Mihaljevič et al., 2019 ; Nazarpour et al., 2019 ; Pelletier et al., 2020 ; Romo-Morales et al., 2020 ; Seleznev et al., 2022 ; Zhao et al., 2019 ). Despite the proven effectiveness of Pb isotope systematics in studying PTE dispersion from mining sites, more research is needed to improve the traceability of PTE related to efflorescence crusts from historical mining sites in arid and semi-arid environments. The present study uses the Pb isotope composition to investigate the traceability of mine tailings and their respective efflorescent salts. A historical mine tailings deposit located in the semi-arid region of northwestern Mexico was selected to address this issue, considering the reported efflorescence salts and high PTE concentrations (Del Rio-Salas et al., 2019 ). The objectives of this investigation were: i) to determine the Pb isotope composition of historical mine tailings and rural dust from surrounding settlements to identify the dispersion of PTE related to the mine tailings deposit, and ii) to determine the Pb isotope composition of the oxide-rich and sulfide-rich tailings materials, as well as their respective efflorescent crusts, to identify similarities with the geogenic end-member and their implications. The findings provide information regarding the dispersion of efflorescent salts and mine tailings materials, the challenges regarding sourcing (geogenic vs. anthropogenic), and the traceability of PTE from historical mine tailings into the surrounding environment. 2. Materials and methods 2.1. Study site San Felipe de Jesús town is located in the Sonora River Basin (northwestern Mexico). Mining, agriculture, and cattle raising represent the most relevant activities in this region. San Felipe de Jesús, a small settlement with ~ 400 inhabitants (INEGI, 2010 ), is neighboring Huépac, Ranchito de Huépac, and Aconchi towns in north-central Sonora; predominant wind directions are north-northeast and south-southwest (Fig. 1 ). A historical small-scale metallurgical facility and a small (~ 140 × ~160 m) mine tailings deposit are located approximately 500 m south of San Felipe de Jesús. The deposit contains ~ 209 tons of waste accumulated since 1920 after the exploitation of skarn mineralization (Ag, Pb, Cu, and Zn) from several small underground mines in the region (Espinoza, 2012 ). The tailings material is fine-grained, unconsolidated, and lacks vegetation, which potentially favors hydric and wind dispersion of material with relatively high concentrations of As (6,213 − 10,098 µg/g), Cu (338–491 µg/g), Mn (16,255 − 29,519 µg/g), Pb (10,464 − 14,161 µg/g), and Zn (8,285 − 60,709 µg/g) to surroundings (Del Rio-Salas et al., 2019 ). The deposit is reddish in the more external parts because of the relative abundance of oxide minerals and grayish in the internal zones because of the relative abundance of sulfide minerals. Development of efflorescent crusts over both types of phases (oxide- and sulfide-rich) materials was observed (Fig. 2 ) and are also characterized by having high concentrations (As: 1,305 − 16,756 µg/g; Cu: 1052-5,691 µg/g; Mn: 41,562 − 117,418 µg/g; Pb: 831-8,672 µg/g; and Zn: 163,909 − 176,218 µg/g) (Del Rio-Salas et al., 2019 ). The most abundant sulfate minerals identified were gypsum, jarosite, kieserite, epsomite, szomolnokite, rozenite, coquimbite, copiapite, starkeyite, beudantite, kieserite, anglesite, among others (Del Rio-Salas et al., 2019 ). More studies have also targeted the study area to determine PTE mobility to the surrounding media (Loredo-Portales et al., 2020 ; Archundia et al., 2021 ), the speciation and oxidation state of Mn (Morales-Pérez et al., 2021 ), and the distribution of heavy metals in surrounding agricultural soils (González‑Méndez et al., 2022). Among the several mining developments along the Sonora River basin, the most outstanding mining zone is located at the northernmost part of the Sonora River basin, represented by the Buenavista del Cobre mine (formerly known as the Cananea mine), the largest porphyry copper mine in Mexico. This mine spilled ~ 40,000 m 3 of Fe-Cu acid solution along the river in 2014 (Calmus et al., 2018 ). After that, several studies assessed the impact (e.g., Díaz-Caravantes et al., 2016 ; Escobar-Quiroz et al., 2019 ; Romero-Lázaro et al., 2019 ; Romo-Morales et al., 2020 ). 2.2. Sample collection and preparation A total of 44 samples were collected for the investigation. Samples from oxide-rich tailings (ORT; n = 8), sulfide-rich tailings (SRT; n = 7), and efflorescent crust collected on both tailings materials (n = 9) were collected from the historical mine tailings near the San Felipe de Jesús town. Moreover, street dust samples were collected from the San Felipe de Jesús (n = 8), Huépac (n = 3), Ranchito de Huépac (n = 1), and Aconchi (n = 3) settlements. Also, agricultural soils (n = 2) from surrounding fields were collected. Additionally, a pyrrhotite sample was collected from the closed El Gachi mine, located ~ 50 km north of the area; this sample was considered in this study since the material that was exploited from this mine was sent to the metallurgical facility of San Felipe de Jesús; therefore, this sample may be representative of the material treated in such facility. A mineralized porphyry rock sample and pyrite sample related to the Cu mineralization from the Buenavista del Cobre mine were collected to compare the Pb isotope signature with the samples from the study area. The oxide- and sulfide-rich mine tailings were collected using a stainless shovel and stored in high-density plastic bags with an airtight seal. Efflorescent crusts were collected using stainless steel tweezers and stored in plastic bottles. Street dust was collected using a broom and dustpan, and samples were stored in high-density plastic bags. The samples were air-dried (if needed) and later were sieved to obtain the fraction < 20 µm; the sieves were ultrasonic cleaned and dried between each sample preparation. The fraction < 20 µm of each sample was powdered using an agate mortar; the mortar was cleaned with powdered quartz and MQ-water before each sample preparation. The sulfide samples were carefully picked and ground using an agate mortar; the mineralized porphyry rock sample was crushed and powdered in a Retsch S100 centrifugal agate ball mill. 2.3. Lead isotope ratios The acids used during the digestion and treatment of samples for measuring Pb isotope ratios were distilled twice, and solutions were prepared with ultrapure Milli-Q water. About 0.5 g of sample (e.g., mine tailings, efflorescent crusts, street dust, sulfide) was digested with aqua regia overnight in Savillex Teflon containers. The rock sample was digested using a mixture of hydrogen fluoride, nitric acid, hydrochloric acid, and perchloric acid. After digestion, the samples were evaporated and reconstituted with 8M HNO 3 for a chromatography procedure using Sr-Spec™ resin. Details on sample treatment and measurements are detailed in Thibodeau et al. ( 2007 ) and Thibodeau et al. ( 2012 ). The Pb isotope ratios were measured in an Inductively Coupled Plasma Mass Spectrometry Multi-collector (MC-ICP-MS) from GV Instruments at the University of Arizona. Precision and accuracy were constrained by using the NBS-981 standard, whose errors during the measurements ranged 206 Pb/ 204 Pb = 16.9405 (± 0.0034–0.0036 2σ), 207 Pb/ 204 Pb = 15.4963 (± 0.0033–0.0038 2σ), and 208 Pb/ 204 Pb = 36.7219 (± 0.0089–0.0099 2σ). 3. Results and Discussion 3.1 Pb isotope composition. The source and dispersion of PTE were assessed using the Pb isotope systematics. Table 1 shows the Pb isotope compositions of the oxide-rich, sulfide-rich, and respective efflorescent crust materials of the historical mine tailings deposit near San Felipe de Jesús town, in addition to the Pb isotope data of street dust collected from surrounding settlements (Fig. 1 ). Table 1 also includes the Pb isotope data from mineralization sample collected in the inactive El Gachi mine, and the available Pb isotope composition of lithological units outcropping in the region reported by González-León et al. ( 2011 ) and González-Becuar et al. ( 2017 ), which are representative of the geogenic component of the area. A clear tendency line is formed (R 2 = 0.9) by the isotope compositions of the mine tailings samples (Fig. 3 ), where the sulfide-rich materials represent the less radiogenic Pb component ( 206 Pb/ 207 Pb≈1.206 and 208 Pb/ 207 Pb≈2.474). In contrast, the more radiogenic member is represented by efflorescence salts and oxide-rich materials ( 206 Pb/ 207 Pb≈1.229 and 208 Pb/ 207 Pb≈2.472). Along this tendency is the isotope composition of efflorescent salts formed over both types of tailings (sulfide- and oxide-rich). The less radiogenic ratios of the sulfide-rich tailings are similar to the Pb isotope composition of a pyrrhotite sample from the inactive El Gachi mine, whose material was processed in the metallurgical facility of the study area. The available Pb isotope data of the lithological units outcropping south and north of the research site are plotted as a reference, whose compositions are the most radiogenic ( 206 Pb/ 207 Pb = 1.219–1.238 and 208 Pb/ 207 Pb = 2.470–2.481; Fig. 3 ) and represent the geochemical background (geogenic end-member) since these rocks are widespread in the region (González-León et al. 2011 ; González-Becuar et al., 2017 ; Calmus et al., 2018 ). The composition of dust collected from surrounding settlements is closely related to the tendency line formed by the mine tailings and efflorescent salts (Fig. 3 ), particularly the dust from San Felipe de Jesús, the nearest settlement to the historical mine tailings. The similarity in the isotope composition may suggest the influence of the mine waste. Moreover, to provide contextualization from the perspective of environmental incidents in the region, the isotopic composition of Pb from the 2014 spill at Buenavista del Cobre mine (Romo-Morales et al., 2020 ) is included in Fig. 3 ; the composition of the spill is less radiogenic than the tendency line defined by the mine tailings, rural dust, and the geogenic component field. Also, Fig. 3 includes the Pb isotope composition of leaded Mexican gasoline (Sañudo-Wilhelmy and Flegal, 1994 ), whose composition is slightly less radiogenic than that of sulfide-rich materials end-member. Moreover, unleaded Mexican gasoline is characterized by a less radiogenic nature (Morton-Bermea et al., 2011 ) (Fig. 3 ). The Pb isotope compositions of Mexican gasoline do not explain the compositions determined in rural dust of studied settlements. The undetermination or exclusion of 204 Pb in environmental studies is common (Komárek et al., 2008 ) and generally leads to simplistic isotope plots (Chong-López et al., 2024 ) that may underestimate or overestimate the influence of geogenic or anthropogenic components. To accurately assess the Pb isotope composition of the studied environmental matrices, Fig. 4 includes the isotope data in terms of 204 Pb. Similarly, the tendency line formed by the mine tailings samples is composed by a less radiogenic end-member represented by the sulfide-rich materials ( 206/204 Pb=18.859–19.113; 207/204 Pb=15.639–15.672; 208/204 Pb=38.693–38.761) whereas the more radiogenic end-member is represented by efflorescence salts and oxide-rich materials ( 206 Pb/ 204 Pb=18.882–19.287; 207 Pb/ 204 Pb=15.642–15.690; 208 Pb/ 204 Pb=38.699–38.792), which is located over the geogenic field (Fig. 4 ). The Pb isotope trend formed by the less radiogenic ratios toward the more radiogenic values can be explained by the oxidation of sulfide minerals that triggered the formation of AMD. The acidification of the tailings materials promoted the release of Pb from sulfides but also from the lithogenic components included in the tailings, such as sediments, minerals, and rock fragments (e.g., altered rocks that are highly susceptible to leaching by AMD). The geogenic component is characterized by higher radiogenic Pb ratios (i.e., geogenic end-member) and is associated with the silicate minerals (i.e., rock forming minerals). Therefore, the linear trend observed in the mine talings materials is the result of mixing between Pb from sulfide-rich materials and lithogenic Pb (Fig. 4 ). An important finding is that the Pb isotope composition of the street dust from San Felipe de Jesús town is intimately associated with the tendency line formed by the isotope compositions of the tailings materials, which support wind dispersion of fine-grained materials from the tailings deposit as previously suggested by the presence of rozenite, a secondary hydrous iron sulfate mineral identified in the tailings deposit and the street dust from San Felipe de Jesús settlement (Del Rio-Salas et al., 2019 ). This evidence supports the dispersion and fate of contaminants related to mine tailings deposits, particularly in arid and semiarid regions, where climate conditions significantly influence the dispersion of materials (Navarro et al., 2008 ; Mokhtari et al., 2018 ; Punia, 2020 ). Excepting one sample from Huépac, the isotope compositions of the street dust samples from Ranchito de Huépac and Huépac settlements, located 5 and 8 km, respectively, northeast of the tailings deposit (Fig. 1 ), are included along the tendency line formed by the mine tailings materials (Figs. 3 and 4 ); the isotope composition supports dispersion along a northeast trend, which is the predominant wind direction (Fig. 1 ). In contrast, the isotope compositions of two street dust samples from Aconchi and one street dust sample from Huépac are not aligned with the tendency line (Fig. 4 ), indicating the influence of additional Pb sources, for instance, from rural and municipal waste, pesticides and herbicides used in agricultural activity, leaded/unleaded gasoline (e.g., Escobar et al., 2013 ; Eichler et al., 2015 ; Civitillo et al., 2016 ; Chrastný et al., 2018 ). The isotope composition of these samples exhibits a subtle inclination toward the Pb isotope compositions of Mexican gasoline (Sañudo-Wilhemly and Flegal, 1994; Morton-Bremea et al., 2011), implying a probable influence. Among the relevant economic activities along the Sonoran River Basin, mining can contribute pollutants to the river plain. The potential contribution can be exacerbated in arid and semiarid regions, particularly during the dry seasons. If river sediments are impacted, suspension of PTE-bearing fine-grained materials can transport pollutants by wind (e.g., Moreno-Rodríguez et al., 2015 ), or impacted sediments can migrate downstream. Considering the upstream spill of the Buenavista del Cobre mine in 2014, Fig. 4 shows that the Pb isotope compositions of the mine spill and impacted sediments are notably different from the studied street dust, indicating the unlikely influence of such spill over the rural dust. Regarding the Pb isotope composition of agricultural soil samples, they are included in the geogenic isotope field (Fig. 4 ), suggesting the close influence of the local lithology and the region's soils. 3.2 Pb traceability from mine tailings deposits. One of the findings of this research highlights the importance of efflorescent salts in terms of metal traceability. Notably, the Pb isotope composition effectively constrains the signature of sulfide-rich tailings and their respective efflorescent salts. In addition, the Pb isotope composition of the efflorescent salts indicates their sensitivity to oxidation and the duration of exposure to weathering. As a result, the longer the tailings have been subjected to weathering, the more oxidized they become, leading to a Pb isotope composition similar to that of the geogenic member, as mixing with geogenic Pb is more likely under such conditions. Therefore, if efflorescent salts are formed from oxidized tailings, Pb involved in the formation of such salts will consist of a Pb mix from sulfide-rich tailings with minerals and rocks from tailings deposits, yielding isotope composition closer to the geogenic end-member (i.e., more radiogenic). In contrast, efflorescent salts formed over the sulfide-rich or slightly oxidized tailings will produce a less radiogenic composition. Pb traceability of efflorescent salts and oxidized mine tailings might be challenging since tailings materials are heterogeneous and geochemically complex matrices. As a consequence of the oxidation processes in arid and semi-arid environments, mine tailings can yield similar isotope composition than the geogenic end-member, which masks compositions and potentially can underestimate the influence of tailings materials over surrounding media (e.g., soils, dust, sediments). Combining mineralogical evidence, metal content, and Pb isotope composition of efflorescent salts will be crucial in accurately identifying the influence of mine tailings on environmental matrices and human health. 4. Conclusions Using the Pb isotope systematics, it is possible to identify the anthropogenic component (less radiogenic), represented by the sulfide-rich materials and respective efflorescent salts. In contrast, the Pb isotope composition of the more oxidized tailings and respective efflorescent salts is more radiogenic, trending through, and similar to the geogenic end-member. The isotope composition of street dust of the nearby settlements suggests the dispersion of the tailings materials to the surroundings. The variability of the Pb isotope composition (from less through more radiogenic) found in the efflorescent salts might be challenging when tracing pollutants in arid and semi-arid environments, especially when the geogenic member conceals the composition. The efflorescence salts in mine tailings from either historical or current mining highlight the importance of assessing the geochemical behavior to establish stabilizing procedures to avoid PTE dispersal to environmental media, considering the hazard represented by the presence of PTE hyperaccumulators and highly soluble efflorescent salts. Therefore, tracking the source, dispersion, and fate of pollutants during environmental assessments of mine-related waste from arid- and semi-arid environments is crucial. Equally important are the government's actions in establishing guidelines (e.g., characterization, mitigation, remediation, regulations) to ensure that efflorescent salts do not pose environmental and health risks. Otherwise, actions should be taken to neutralize, prevent the formation, and systematically monitor the sites of concern. Declarations -Funding This research was supported by project IN113519 (PAPIIT-UNAM), granted to Del Rio-Salas, CESUES-PTC-035 (NPCT-PRODEP), granted to Moreno-Rodríguez, and CONAHCYT-300409, granted to Loredo-Portales. - Competing Interests All authors have non-financial interests to disclose. - Conflict of interests Authors declare that they have no conflict of interest. -Authors Contributions All authors contributed to the study conception and design and approved the final version of the manuscript. Rafael Del Rio-Salas: conception, research design, acquisition of data, analysis, interpretation, writing original draft, review, editing. Verónica Moreno-Rodríguez: research design, interpretation, writing original draft, review. René Loredo-Portales: analysis, interpretation, writing original draft, review. Sergio Adrián Salgado-Souto: analysis, interpretation, writing original draft, review, editing. Martín Valencia-Moreno: interpretation, review, editing. Lucas Ochoa-Landín: interpretation, review, editing. Diana Romo-Morales: acquisition of data, analysis, review, editing. -Ethics Approval Not applicable -Consent to Participate Not applicable -Consent to Publish Not applicable Acknowledgments This investigation was supported by project IN113519 (PAPIIT-UNAM) granted to Del Rio-Salas, CESUES-PTC-035 (NPCT-PRODEP), and CONAHCYT-300409. We thank Mark Baker for his valuable assistance during Pb isotope ratio measurements. We are thankful to J.F. Martínez Rodríguez, A. Vázquez-Salgado, L.G. Martínez-Jardines, and D. Ramos Pérez for laboratory support. We thank A. Orcí Romero for preparation of mineralization samples. We thank the CONAHCYT National Laboratories calls, the Laboratorio Nacional de Geoquímica y Mineralogía-LANGEM, and Laboratorio de Ciencias Ambientales de la ERNO. References Archundia, D., Prado-Pano, B., González-Méndez, B., Loredo-Portales, R., Molina-Freaner, F. (2021). 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Loredo-Portales, R., Bustamante-Arce, J., González-Villa, H. N., Moreno-Rodríguez, V., Del Rio-Salas, R., Molina-Freaner, F., et al., (2020). Mobility and accessibility of Zn, Pb, and As in abandoned mine tailings of northwestern Mexico. Environmental Science and Pollution Research, 27(21), 26605–26620. Lottermoser., B. (2010). Mine Wastes. Springer Science & Business Media. Lottermoser, B. (2017). Environmental indicators in metal mining. Springer International Publishing. Martínez-López, S., Martínez-Sánchez, M. J., & Pérez-Sirvent, C. (2021). Do old mining areas represent an environmental problem and health risk? A critical discussion through a particular case. Minerals, 11(6), 594. McPartland, M., Garbus, S. E., Lierhagen, S., Sonne, C., Krøkje, Å. (2020). Lead isotopic signatures in blood from incubating common eiders (Somateria mollissima) in the central Baltic Sea. Environment International, 142, 105874. Mihaljevič, M., Baieta, R., Ettler, V., Vaněk, A., Kříbek, B., Penížek, V., Drahota, P., Trubač, J., Sracek, O., Chrastný, V., Mapani, B. S. (2019). Tracing the metal dynamics in semi-arid soils near mine tailings using stable Cu and Pb isotopes. Chemical Geology, 515, 61–76. Mokhtari, A. R., Feiznia, S., Jafari, M., Tavili, A., Ghaneei-Bafghi, M. J., Rahmany, F., Kerry, R. (2018). Investigating the role of wind in the dispersion of heavy metals around mines in arid regions (a case study from Kushk Pb–Zn Mine, Bafgh, Iran). Bulletin of environmental contamination and toxicology, 101(1), 124–130. Morales-Pérez, A., Moreno-Rodríguez, V., Del Rio-Salas, R., Imam, N. G., González-Méndez, B., Pi-Puig, T., et al., (2021). Geochemical changes of Mn in contaminated agricultural soils nearby historical mine tailings: Insights from XAS, XRD and, SEP. Chemical Geology, 573, 120217. Moreno-Rodríguez, V., Del Rio-Salas, R., Adams, D. K., Ochoa-Landin, L., Zepeda, J., Gómez-Alvarez, A., ... & Meza-Figueroa, D. (2015). Historical trends and sources of TSP in a Sonoran desert city: Can the North America Monsoon enhance dust emissions?. Atmospheric Environment, 110, 111-121. Morton-Bermea, O., Rodríguez-Salazar, M. T., Hernández-Alvarez, E., García-Arreola, M. E., Lozano-Santacruz, R. (2011). Lead isotopes as tracers of anthropogenic pollution in urban topsoils of Mexico City. Geochemistry, 71(2), 189–195. Navarro, M. C., Pérez-Sirvent, C., Martínez-Sánchez, M. J., Vidal, J., Tovar, P. J., Bech, J. (2008). Abandoned mine sites as a source of contamination by heavy metals: a case study in a semi-arid zone. Journal of Geochemical Exploration, 96(2-3), 183–193. Nazarpour, A., Watts, M. J., Madhani, A., Elahi, S. (2019). Source, spatial distribution and pollution assessment of Pb, Zn, Cu, and Pb, isotopes in urban soils of Ahvaz City, a semi-arid metropolis in southwest Iran. Scientific reports, 9(1), 1–11. Pelletier, N., Chételat, J., Cousens, B., Zhang, S., Stepner, D., Muir, D. C., Vermaire, J. C. (2020). Lead contamination from gold mining in Yellowknife Bay (Northwest Territories), reconstructed using stable lead isotopes. Environmental Pollution, 259, 113888. Peña-Ortega, M., Del Rio-Salas, R., Valencia-Sauceda, J., Mendívil-Quijada, H., Minjarez-Osorio, C., Molina-Freaner, F., ... & Moreno-Rodríguez, V. (2019). Environmental assessment and historic erosion calculation of abandoned mine tailings from a semi-arid zone of northwestern Mexico: insights from geochemistry and unmanned aerial vehicles. Environmental Science and Pollution Research, 26, 26203-26215. Pérez-Sirvent, C., Hernández-Pérez, C., Martínez-Sánchez, M. J., García-Lorenzo, M. L., & Bech, J. (2016). Geochemical characterisation of surface waters, topsoils and efflorescences in a historic metal-mining area in Spain. Journal of soils and sediments, 16, 1238-1252. Punia, A. (2020). Role of temperature, wind, and precipitation in heavy metal contamination at copper mines: a review. Environmental Science and Pollution Research, 1-17. Romero-Lázaro, E. M., Ramos-Pérez, D., Romero, F. M., & Sedov, S. (2019). Indicadores indirectos de contaminación residual en suelos y sedimentos de la cuenca del Río Sonora, México. Revista internacional de contaminación ambiental, 35(2), 371-386. Romo-Morales, D., Moreno-Rodríguez, V., Molina-Freaner, F., Valencia-Moreno, M., Ruiz, J., Minjárez-Osorio, C., Hernández-Mindiola, E., Del Rio-Salas, R. (2020). Assessment of Geogenic and Anthropogenic Pollution Sources Using an Aquatic Plant Along the Sonora River Basin: Insights from Elemental Concentrations and Pb Isotope Signatures. Natural Resources Research, 1–14. Sañudo-Wilhelmy, S.A., Flegal, A.R. (1994). Temporal variations in lead concentrations and isotopic composition in the Southern California Bight. Geochimica et Cosmochimica Acta, 58(15), 3315–3320. Seleznev, A., Yarmoshenko, I., Malinovsky, G., Ilgasheva, E., Chervyakovskaya, M., Streletskaya, M., Kiseleva, D. (2022). Lead isotope ratios in urban surface deposited sediments as an indicator of urban geochemical transformation: Example of Russian cities. Applied Geochemistry, 137, 105184. Thibodeau, A. M., Killick, D. J., Ruiz, J., Chesley, J. T., Deagan, K., Cruxent, J. M., Lyman, W. (2007). The strange case of the earliest silver extraction by European colonists in the New World. Proceedings of the National Academy of Sciences, 104(9), 3663-3666. Thibodeau, A. M., Chesley, J. T., Ruiz, J. (2012). Lead isotope analysis as a new method for identifying material culture belonging to the Vázquez de Coronado expedition. Journal of Archaeological Science, 39(1), 58–66. Zhao, L., Hu, G., Yan, Y., Yu, R., Cui, J., Wang, X., Yan, Y. (2019). Source apportionment of heavy metals in urban road dust in a continental city of eastern China: Using Pb and Sr isotopes combined with multivariate statistical analysis. Atmospheric Environment, 201, 201–211. Table 1 Table 1 is available in the Supplementary Files section. Additional Declarations No competing interests reported. Supplementary Files Table1.pdf Table 1. Lead isotope compositions of historical mine tailings, efflorescent crusts, and street dust of San Felipe de Jesús area, and mineralized and other environmental matrices of the region, in northwestern Mexico. Note: SRT, sulfide-rich tailings; ORT, oxide-rich tailings; BCM, Buenavista del Cobre mine; Ma, million years. Cite Share Download PDF Status: Published Journal Publication published 24 Aug, 2024 Read the published version in Environmental Geochemistry and Health → Version 1 posted Editorial decision: Revision requested 24 Jun, 2024 Editor assigned by journal 24 Jun, 2024 Submission checks completed at journal 20 Jun, 2024 First submitted to journal 19 Jun, 2024 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-4608395","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":318216199,"identity":"a9627532-8888-4c73-b8b2-752bb1e04f93","order_by":0,"name":"Rafael Del Rio-Salas","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA8UlEQVRIiWNgGAWjYFCCBMYDDAZAmh2IPwAxGzthLQwQLcwMDIwzQFqYidLCANHCzANl4AXm7ckHDlcU2NjzNzM//mzza5s8HzMD44ePObi1yJx5lnDwjEFa4ozDbGbSuX23DduYGZglZ27DrUVCIsfgYIPB4QSGwwxmzLk9txmBWtiYefFqyf8A0mIvf5j982fLntv2RGjJYQBpYdxwmMdAmuHH7UTCWniegRyWlrjxME+ZZG/D7eQ2ZsZm/H5hT374sOGPjb3c8fbNH378uW07v7354IePeLSgAsY2MNlArHoQ+EOK4lEwCkbBKBgpAAA7SVAG1HKDrAAAAABJRU5ErkJggg==","orcid":"","institution":"Universidad Nacional Autónoma de México","correspondingAuthor":true,"prefix":"","firstName":"Rafael","middleName":"Del","lastName":"Rio-Salas","suffix":""},{"id":318216200,"identity":"b4ede048-d376-472b-852d-44ea544ce4df","order_by":1,"name":"Verónica Moreno-Rodríguez","email":"","orcid":"","institution":"Universidad Estatal de Sonora","correspondingAuthor":false,"prefix":"","firstName":"Verónica","middleName":"","lastName":"Moreno-Rodríguez","suffix":""},{"id":318216201,"identity":"af779528-de6a-450a-ad8f-4858c7e54d6f","order_by":2,"name":"René Loredo-Portales","email":"","orcid":"","institution":"Universidad Nacional Autónoma de México","correspondingAuthor":false,"prefix":"","firstName":"René","middleName":"","lastName":"Loredo-Portales","suffix":""},{"id":318216202,"identity":"f6a3af32-4e50-4da1-b150-7f5b3838e26b","order_by":3,"name":"Sergio Adrián Salgado-Souto","email":"","orcid":"","institution":"Universidad Autónoma de Guerrero","correspondingAuthor":false,"prefix":"","firstName":"Sergio","middleName":"Adrián","lastName":"Salgado-Souto","suffix":""},{"id":318216203,"identity":"cebb1a0f-62c7-4b36-87a6-7982c3543b79","order_by":4,"name":"Martín Valencia-Moreno","email":"","orcid":"","institution":"Universidad Nacional Autónoma de México","correspondingAuthor":false,"prefix":"","firstName":"Martín","middleName":"","lastName":"Valencia-Moreno","suffix":""},{"id":318216204,"identity":"d38a5e11-7c80-4ee8-a295-7535c9c0fcf4","order_by":5,"name":"Lucas Ochoa-Landín","email":"","orcid":"","institution":"Universidad de Sonora","correspondingAuthor":false,"prefix":"","firstName":"Lucas","middleName":"","lastName":"Ochoa-Landín","suffix":""},{"id":318216205,"identity":"e03894c9-5d31-4c58-bcb6-ef58d35aa945","order_by":6,"name":"Diana Romo-Morales","email":"","orcid":"","institution":"Universidad de Sonora","correspondingAuthor":false,"prefix":"","firstName":"Diana","middleName":"","lastName":"Romo-Morales","suffix":""}],"badges":[],"createdAt":"2024-06-20 01:24:37","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4608395/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4608395/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1007/s10653-024-02180-3","type":"published","date":"2024-08-24T15:57:21+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":60086551,"identity":"e3bc4223-f2d0-43b6-992a-9003456d3b49","added_by":"auto","created_at":"2024-07-11 15:00:07","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":4567445,"visible":true,"origin":"","legend":"\u003cp\u003eMap depicting the location and sampling points of San Felipe de Jesús area and nearby towns in central Sonora, Mexico. SRB: Sonora River Basin.\u003c/p\u003e","description":"","filename":"Figure1.png","url":"https://assets-eu.researchsquare.com/files/rs-4608395/v1/0fddb7c052b9893619524fce.png"},{"id":60086951,"identity":"184a9597-9e8e-42a4-9ad9-444c12acbe1d","added_by":"auto","created_at":"2024-07-11 15:08:07","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":3851107,"visible":true,"origin":"","legend":"\u003cp\u003ePictures depicting some features of the historical mine tailings near San Felipe de Jesús settlement. a) Sulfide-rich (lower part) and oxide-rich (upper part) tailings; note the development of efflorescent crusts (white crusts) over the sulfide-rich materials. b) view of the tailings deposit with efflorescent crusts developed over the surface. c) active agricultural soils next to the tailings deposit. d) road next to tailings deposit that connects to the San Felipe de Jesús town.\u003c/p\u003e","description":"","filename":"Figure2.png","url":"https://assets-eu.researchsquare.com/files/rs-4608395/v1/9acef9b420a9939b498a11c9.png"},{"id":60087569,"identity":"1dd65aaf-e899-4363-b6c8-49941a8283b7","added_by":"auto","created_at":"2024-07-11 15:16:07","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":40199,"visible":true,"origin":"","legend":"\u003cp\u003e\u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e207\u003c/sup\u003ePb vs. \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e207\u003c/sup\u003ePb diagram showing the composition of historical mine tailings from San Felipe de Jesús and street dust from nearby settlements. The geogenic end-member field is shown according to the representative lithology of the study area (González-León et al., 2011; González-Becuar et al., 2017). Also shown is the isotope data of the 2014 Buenavista del Cobre mine spill (Romo-Morales et al. (2019) and unleaded (Morton-Bermea et al., 2011) and leaded (Sañudo-Wilhelmy and Flegal, 1994) Mexican gasoline.\u003c/p\u003e","description":"","filename":"Figure3.png","url":"https://assets-eu.researchsquare.com/files/rs-4608395/v1/09200f75c62217090792a7a4.png"},{"id":60086554,"identity":"eed3daf8-40cf-4dc7-aeac-cb541adbedab","added_by":"auto","created_at":"2024-07-11 15:00:07","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":62608,"visible":true,"origin":"","legend":"\u003cp\u003e\u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb vs. \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb and \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb vs. \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb diagrams of historical mine tailings from San Felipe de Jesús and street dust from surrounding settlements. The geogenic end-member field is shown according to the representative lithology of the study area (González-León et al., 2011; González-Becuar et al., 2017). Also shown is the isotope data of the 2014 Buenavista del Cobre mine spill (Romo-Morales et al. (2019) and unleaded (Morton-Bermea et al., 2011) and leaded (Sañudo-Wilhelmy and Flegal, 1994) Mexican gasoline.\u003c/p\u003e","description":"","filename":"Figure4.png","url":"https://assets-eu.researchsquare.com/files/rs-4608395/v1/44633ae8b1861154828e8663.png"},{"id":63300632,"identity":"ce0a3be3-6d11-454e-91fe-01f4498014b1","added_by":"auto","created_at":"2024-08-26 16:15:57","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":13239968,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4608395/v1/2ec2646f-bdaa-4c99-aa73-77df5fa33040.pdf"},{"id":60086555,"identity":"78552f91-d4e1-4451-8ca0-3e28e41e3259","added_by":"auto","created_at":"2024-07-11 15:00:07","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":61928,"visible":true,"origin":"","legend":"\u003cp\u003eTable 1. Lead isotope compositions of historical mine tailings, efflorescent crusts, and street dust of San Felipe de Jesús area, and mineralized and other environmental matrices of the region, in northwestern Mexico.\u003c/p\u003e\n\u003cp\u003eNote: SRT, sulfide-rich tailings; ORT, oxide-rich tailings; BCM, Buenavista del Cobre mine; Ma, million years.\u003c/p\u003e","description":"","filename":"Table1.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4608395/v1/884d2cebd3124f967817def0.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"Traceability and dispersion of highly toxic soluble phases from historical mine tailings","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eEfflorescence salts are naturally occurring secondary minerals in various environments, including mine waste. In the context of mine waste, the efflorescent salts can accumulate and momentarily immobilize metals, which can be released later in solution, as they commonly consist of highly soluble phases (Lottermoser, \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e2017\u003c/span\u003e). Additionally, efflorescent salts are characterized by low cohesion and density, facilitating decrepitation, lifting, and wind dispersion (Del Rio-Salas et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Punia, 2021). Therefore, although ephemeral, they are quite effective in dispersing potential toxic elements (PTE) into the environment.\u003c/p\u003e \u003cp\u003eAmong the different types of mine waste (mining, mineral processing, metallurgical, etc.), mine tailings impoundments are considered the largest and most dangerous industrial infrastructures worldwide (Davies, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e2002\u003c/span\u003e). Mine tailings are constructed to confine the waste during the mine\u0026rsquo;s operational life and after closure. They contain fine-grained materials, including minerals, rock fragments, sediments, chemical reactants, and water. Tailings impoundments generated during historical mining commonly contain higher PTE contents than those from active mines due to less efficient metallurgical processes and laxer environmental standards at the time, among other reasons (e.g., Del Rio-Salas et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). Particularly in developing countries, historical tailings impoundments lack containment, monitoring, and remediation programs and have become part of the landscape (e.g., Pe\u0026ntilde;a-Ortega et al., \u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e2019\u003c/span\u003e).\u003c/p\u003e \u003cp\u003ePTE content in historical mine tailings is related to metal commodities allocated within sulfide minerals after processing. Exposure to air and humidity triggers the breakdown of sulfides through oxidation processes, producing acidic waters enriched in sulfate and PTE, a phenomenon widely known as acid mine drainage (AMD) (Lottermoser, \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e2010\u003c/span\u003e; \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e2017\u003c/span\u003e). AMD is critical in arid and semi-arid environments since high temperatures, torrential rains, high evaporation rates, and capillarity action favor the migration of PTE-bearing fluids to the tailings surface, precipitating the efflorescent salts (Khorasanipour, \u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e2015\u003c/span\u003e) composed mainly by sulfates, in addition to chlorides, nitrates, among other mineral species.\u003c/p\u003e \u003cp\u003eUnderstanding the dispersion of tailings materials and efflorescent salts is essential not only because of their high capacity to contaminate different environmental media such as soil, water, and dust but also because of their high potential toxicity to humans (Gonzalez et al., 2014; P\u0026eacute;rez-Sirvent et al., \u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e2016\u003c/span\u003e; Loredo-Jasso et al., \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Mart\u0026iacute;nez-L\u0026oacute;pez et al., \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Punia 2021). Specifically, efflorescent salts and relatively high PTE contents related to mine tailings have been identified in sediments (Garc\u0026iacute;a-Lorenzo et al., \u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e2012\u003c/span\u003e) and dust from rural settlements near historical mining sites (Del Rio-Salas et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). In the latter scenario, rural dust can serve as the final fate for PTE associated with mine tailings and efflorescent salts; detecting efflorescent salts and high PTE concentration in rural dust underscores their dispersal capacity despite their temporary nature.\u003c/p\u003e \u003cp\u003eAmong different techniques to assess dispersion, Pb isotope systematics has effectively traced Pb in various research fields, including petrogenesis, tectonics, ore deposits, anthropology, forensic sciences, environmental sciences, etc. Lead has four naturally occurring stable isotopes (\u003csup\u003e204\u003c/sup\u003ePb, \u003csup\u003e206\u003c/sup\u003ePb, \u003csup\u003e207\u003c/sup\u003ePb, and \u003csup\u003e208\u003c/sup\u003ePb); \u003csup\u003e204\u003c/sup\u003ePb is non-radiogenic, while \u003csup\u003e206\u003c/sup\u003ePb, \u003csup\u003e207\u003c/sup\u003ePb, and \u003csup\u003e208\u003c/sup\u003ePb are the decay products of \u003csup\u003e238\u003c/sup\u003eU, \u003csup\u003e235\u003c/sup\u003eU, and \u003csup\u003e232\u003c/sup\u003eTh, respectively (Dickin, \u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e1995\u003c/span\u003e). Lead does not fractionate, and particularly in environmental studies, processes such as emission, transport, and deposition do not affect the isotope composition, enabling source identification (geogenic \u003cem\u003evs.\u003c/em\u003e anthropogenic) and tracing dispersion of PTE in environmental media (e.g., dust, particulate matter, soils, sediments, plants, mine waste) and organisms (i.e., Dong et al., \u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Fry et al., \u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Lee et al., \u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; McPartland et al., \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Mihaljevič et al., \u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Nazarpour et al., \u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Pelletier et al., \u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Romo-Morales et al., \u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Seleznev et al., \u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e2022\u003c/span\u003e; Zhao et al., \u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e2019\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eDespite the proven effectiveness of Pb isotope systematics in studying PTE dispersion from mining sites, more research is needed to improve the traceability of PTE related to efflorescence crusts from historical mining sites in arid and semi-arid environments. The present study uses the Pb isotope composition to investigate the traceability of mine tailings and their respective efflorescent salts. A historical mine tailings deposit located in the semi-arid region of northwestern Mexico was selected to address this issue, considering the reported efflorescence salts and high PTE concentrations (Del Rio-Salas et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). The objectives of this investigation were: i) to determine the Pb isotope composition of historical mine tailings and rural dust from surrounding settlements to identify the dispersion of PTE related to the mine tailings deposit, and ii) to determine the Pb isotope composition of the oxide-rich and sulfide-rich tailings materials, as well as their respective efflorescent crusts, to identify similarities with the geogenic end-member and their implications. The findings provide information regarding the dispersion of efflorescent salts and mine tailings materials, the challenges regarding sourcing (geogenic vs. anthropogenic), and the traceability of PTE from historical mine tailings into the surrounding environment.\u003c/p\u003e"},{"header":"2. Materials and methods","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1. Study site\u003c/h2\u003e \u003cp\u003eSan Felipe de Jes\u0026uacute;s town is located in the Sonora River Basin (northwestern Mexico). Mining, agriculture, and cattle raising represent the most relevant activities in this region. San Felipe de Jes\u0026uacute;s, a small settlement with ~\u0026thinsp;400 inhabitants (INEGI, \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e2010\u003c/span\u003e), is neighboring Hu\u0026eacute;pac, Ranchito de Hu\u0026eacute;pac, and Aconchi towns in north-central Sonora; predominant wind directions are north-northeast and south-southwest (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e). A historical small-scale metallurgical facility and a small (~\u0026thinsp;140 \u0026times; ~160 m) mine tailings deposit are located approximately 500 m south of San Felipe de Jes\u0026uacute;s. The deposit contains\u0026thinsp;~\u0026thinsp;209 tons of waste accumulated since 1920 after the exploitation of skarn mineralization (Ag, Pb, Cu, and Zn) from several small underground mines in the region (Espinoza, \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e2012\u003c/span\u003e). The tailings material is fine-grained, unconsolidated, and lacks vegetation, which potentially favors hydric and wind dispersion of material with relatively high concentrations of As (6,213\u0026thinsp;\u0026minus;\u0026thinsp;10,098 \u0026micro;g/g), Cu (338\u0026ndash;491 \u0026micro;g/g), Mn (16,255\u0026thinsp;\u0026minus;\u0026thinsp;29,519 \u0026micro;g/g), Pb (10,464\u0026thinsp;\u0026minus;\u0026thinsp;14,161 \u0026micro;g/g), and Zn (8,285\u0026thinsp;\u0026minus;\u0026thinsp;60,709 \u0026micro;g/g) to surroundings (Del Rio-Salas et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). The deposit is reddish in the more external parts because of the relative abundance of oxide minerals and grayish in the internal zones because of the relative abundance of sulfide minerals. Development of efflorescent crusts over both types of phases (oxide- and sulfide-rich) materials was observed (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e) and are also characterized by having high concentrations (As: 1,305\u0026thinsp;\u0026minus;\u0026thinsp;16,756 \u0026micro;g/g; Cu: 1052-5,691 \u0026micro;g/g; Mn: 41,562\u0026thinsp;\u0026minus;\u0026thinsp;117,418 \u0026micro;g/g; Pb: 831-8,672 \u0026micro;g/g; and Zn: 163,909\u0026thinsp;\u0026minus;\u0026thinsp;176,218 \u0026micro;g/g) (Del Rio-Salas et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). The most abundant sulfate minerals identified were gypsum, jarosite, kieserite, epsomite, szomolnokite, rozenite, coquimbite, copiapite, starkeyite, beudantite, kieserite, anglesite, among others (Del Rio-Salas et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). More studies have also targeted the study area to determine PTE mobility to the surrounding media (Loredo-Portales et al., \u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e2020\u003c/span\u003e; Archundia et al., \u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e2021\u003c/span\u003e), the speciation and oxidation state of Mn (Morales-P\u0026eacute;rez et al., \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e2021\u003c/span\u003e), and the distribution of heavy metals in surrounding agricultural soils (Gonz\u0026aacute;lez‑M\u0026eacute;ndez et al., 2022).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAmong the several mining developments along the Sonora River basin, the most outstanding mining zone is located at the northernmost part of the Sonora River basin, represented by the Buenavista del Cobre mine (formerly known as the Cananea mine), the largest porphyry copper mine in Mexico. This mine spilled\u0026thinsp;~\u0026thinsp;40,000 m\u003csup\u003e3\u003c/sup\u003e of Fe-Cu acid solution along the river in 2014 (Calmus et al., \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2018\u003c/span\u003e). After that, several studies assessed the impact (e.g., D\u0026iacute;az-Caravantes et al., \u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e2016\u003c/span\u003e; Escobar-Quiroz et al., \u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Romero-L\u0026aacute;zaro et al., \u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Romo-Morales et al., \u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e2020\u003c/span\u003e).\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2. Sample collection and preparation\u003c/h2\u003e \u003cp\u003eA total of 44 samples were collected for the investigation. Samples from oxide-rich tailings (ORT; n\u0026thinsp;=\u0026thinsp;8), sulfide-rich tailings (SRT; n\u0026thinsp;=\u0026thinsp;7), and efflorescent crust collected on both tailings materials (n\u0026thinsp;=\u0026thinsp;9) were collected from the historical mine tailings near the San Felipe de Jes\u0026uacute;s town. Moreover, street dust samples were collected from the San Felipe de Jes\u0026uacute;s (n\u0026thinsp;=\u0026thinsp;8), Hu\u0026eacute;pac (n\u0026thinsp;=\u0026thinsp;3), Ranchito de Hu\u0026eacute;pac (n\u0026thinsp;=\u0026thinsp;1), and Aconchi (n\u0026thinsp;=\u0026thinsp;3) settlements. Also, agricultural soils (n\u0026thinsp;=\u0026thinsp;2) from surrounding fields were collected. Additionally, a pyrrhotite sample was collected from the closed El Gachi mine, located\u0026thinsp;~\u0026thinsp;50 km north of the area; this sample was considered in this study since the material that was exploited from this mine was sent to the metallurgical facility of San Felipe de Jes\u0026uacute;s; therefore, this sample may be representative of the material treated in such facility. A mineralized porphyry rock sample and pyrite sample related to the Cu mineralization from the Buenavista del Cobre mine were collected to compare the Pb isotope signature with the samples from the study area.\u003c/p\u003e \u003cp\u003eThe oxide- and sulfide-rich mine tailings were collected using a stainless shovel and stored in high-density plastic bags with an airtight seal. Efflorescent crusts were collected using stainless steel tweezers and stored in plastic bottles. Street dust was collected using a broom and dustpan, and samples were stored in high-density plastic bags. The samples were air-dried (if needed) and later were sieved to obtain the fraction\u0026thinsp;\u0026lt;\u0026thinsp;20 \u0026micro;m; the sieves were ultrasonic cleaned and dried between each sample preparation. The fraction\u0026thinsp;\u0026lt;\u0026thinsp;20 \u0026micro;m of each sample was powdered using an agate mortar; the mortar was cleaned with powdered quartz and MQ-water before each sample preparation. The sulfide samples were carefully picked and ground using an agate mortar; the mineralized porphyry rock sample was crushed and powdered in a Retsch S100 centrifugal agate ball mill.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3. Lead isotope ratios\u003c/h2\u003e \u003cp\u003eThe acids used during the digestion and treatment of samples for measuring Pb isotope ratios were distilled twice, and solutions were prepared with ultrapure Milli-Q water. About 0.5 g of sample (e.g., mine tailings, efflorescent crusts, street dust, sulfide) was digested with aqua regia overnight in Savillex Teflon containers. The rock sample was digested using a mixture of hydrogen fluoride, nitric acid, hydrochloric acid, and perchloric acid. After digestion, the samples were evaporated and reconstituted with 8M HNO\u003csub\u003e3\u003c/sub\u003e for a chromatography procedure using Sr-Spec\u0026trade; resin. Details on sample treatment and measurements are detailed in Thibodeau et al. (\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e2007\u003c/span\u003e) and Thibodeau et al. (\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e2012\u003c/span\u003e). The Pb isotope ratios were measured in an Inductively Coupled Plasma Mass Spectrometry Multi-collector (MC-ICP-MS) from GV Instruments at the University of Arizona. Precision and accuracy were constrained by using the NBS-981 standard, whose errors during the measurements ranged \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb = 16.9405 (\u0026plusmn;\u0026thinsp;0.0034\u0026ndash;0.0036 2σ), \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb = 15.4963 (\u0026plusmn;\u0026thinsp;0.0033\u0026ndash;0.0038 2σ), and \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb = 36.7219 (\u0026plusmn;\u0026thinsp;0.0089\u0026ndash;0.0099 2σ).\u003c/p\u003e \u003c/div\u003e"},{"header":"3. Results and Discussion","content":"\u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e3.1 Pb isotope composition.\u003c/h2\u003e \u003cp\u003eThe source and dispersion of PTE were assessed using the Pb isotope systematics. Table\u0026nbsp;1 shows the Pb isotope compositions of the oxide-rich, sulfide-rich, and respective efflorescent crust materials of the historical mine tailings deposit near San Felipe de Jes\u0026uacute;s town, in addition to the Pb isotope data of street dust collected from surrounding settlements (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e). Table\u0026nbsp;1 also includes the Pb isotope data from mineralization sample collected in the inactive El Gachi mine, and the available Pb isotope composition of lithological units outcropping in the region reported by Gonz\u0026aacute;lez-Le\u0026oacute;n et al. (\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e2011\u003c/span\u003e) and Gonz\u0026aacute;lez-Becuar et al. (\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e2017\u003c/span\u003e), which are representative of the geogenic component of the area.\u003c/p\u003e \u003cp\u003eA clear tendency line is formed (R\u003csup\u003e2\u003c/sup\u003e\u0026thinsp;=\u0026thinsp;0.9) by the isotope compositions of the mine tailings samples (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e), where the sulfide-rich materials represent the less radiogenic Pb component (\u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e207\u003c/sup\u003ePb\u0026asymp;1.206 and \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e207\u003c/sup\u003ePb\u0026asymp;2.474). In contrast, the more radiogenic member is represented by efflorescence salts and oxide-rich materials (\u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e207\u003c/sup\u003ePb\u0026asymp;1.229 and \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e207\u003c/sup\u003ePb\u0026asymp;2.472). Along this tendency is the isotope composition of efflorescent salts formed over both types of tailings (sulfide- and oxide-rich). The less radiogenic ratios of the sulfide-rich tailings are similar to the Pb isotope composition of a pyrrhotite sample from the inactive El Gachi mine, whose material was processed in the metallurgical facility of the study area. The available Pb isotope data of the lithological units outcropping south and north of the research site are plotted as a reference, whose compositions are the most radiogenic (\u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e207\u003c/sup\u003ePb =\u0026thinsp;1.219\u0026ndash;1.238 and \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e207\u003c/sup\u003ePb =\u0026thinsp;2.470\u0026ndash;2.481; Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e) and represent the geochemical background (geogenic end-member) since these rocks are widespread in the region (Gonz\u0026aacute;lez-Le\u0026oacute;n et al. \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e2011\u003c/span\u003e; Gonz\u0026aacute;lez-Becuar et al., \u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e2017\u003c/span\u003e; Calmus et al., \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2018\u003c/span\u003e). The composition of dust collected from surrounding settlements is closely related to the tendency line formed by the mine tailings and efflorescent salts (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e), particularly the dust from San Felipe de Jes\u0026uacute;s, the nearest settlement to the historical mine tailings. The similarity in the isotope composition may suggest the influence of the mine waste.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eMoreover, to provide contextualization from the perspective of environmental incidents in the region, the isotopic composition of Pb from the 2014 spill at Buenavista del Cobre mine (Romo-Morales et al., \u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e2020\u003c/span\u003e) is included in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e; the composition of the spill is less radiogenic than the tendency line defined by the mine tailings, rural dust, and the geogenic component field. Also, Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e includes the Pb isotope composition of leaded Mexican gasoline (Sa\u0026ntilde;udo-Wilhelmy and Flegal, \u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e1994\u003c/span\u003e), whose composition is slightly less radiogenic than that of sulfide-rich materials end-member. Moreover, unleaded Mexican gasoline is characterized by a less radiogenic nature (Morton-Bermea et al., \u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e2011\u003c/span\u003e) (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e). The Pb isotope compositions of Mexican gasoline do not explain the compositions determined in rural dust of studied settlements.\u003c/p\u003e \u003cp\u003eThe undetermination or exclusion of \u003csup\u003e204\u003c/sup\u003ePb in environmental studies is common (Kom\u0026aacute;rek et al., \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e2008\u003c/span\u003e) and generally leads to simplistic isotope plots (Chong-L\u0026oacute;pez et al., \u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e2024\u003c/span\u003e) that may underestimate or overestimate the influence of geogenic or anthropogenic components. To accurately assess the Pb isotope composition of the studied environmental matrices, Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e includes the isotope data in terms of \u003csup\u003e204\u003c/sup\u003ePb. Similarly, the tendency line formed by the mine tailings samples is composed by a less radiogenic end-member represented by the sulfide-rich materials (\u003csup\u003e206/204\u003c/sup\u003ePb=18.859\u0026ndash;19.113; \u003csup\u003e207/204\u003c/sup\u003ePb=15.639\u0026ndash;15.672; \u003csup\u003e208/204\u003c/sup\u003ePb=38.693\u0026ndash;38.761) whereas the more radiogenic end-member is represented by efflorescence salts and oxide-rich materials (\u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb=18.882\u0026ndash;19.287; \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb=15.642\u0026ndash;15.690; \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb=38.699\u0026ndash;38.792), which is located over the geogenic field (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe Pb isotope trend formed by the less radiogenic ratios toward the more radiogenic values can be explained by the oxidation of sulfide minerals that triggered the formation of AMD. The acidification of the tailings materials promoted the release of Pb from sulfides but also from the lithogenic components included in the tailings, such as sediments, minerals, and rock fragments (e.g., altered rocks that are highly susceptible to leaching by AMD). The geogenic component is characterized by higher radiogenic Pb ratios (i.e., geogenic end-member) and is associated with the silicate minerals (i.e., rock forming minerals). Therefore, the linear trend observed in the mine talings materials is the result of mixing between Pb from sulfide-rich materials and lithogenic Pb (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eAn important finding is that the Pb isotope composition of the street dust from San Felipe de Jes\u0026uacute;s town is intimately associated with the tendency line formed by the isotope compositions of the tailings materials, which support wind dispersion of fine-grained materials from the tailings deposit as previously suggested by the presence of rozenite, a secondary hydrous iron sulfate mineral identified in the tailings deposit and the street dust from San Felipe de Jes\u0026uacute;s settlement (Del Rio-Salas et al., \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). This evidence supports the dispersion and fate of contaminants related to mine tailings deposits, particularly in arid and semiarid regions, where climate conditions significantly influence the dispersion of materials (Navarro et al., \u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e2008\u003c/span\u003e; Mokhtari et al., \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e2018\u003c/span\u003e; Punia, \u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). Excepting one sample from Hu\u0026eacute;pac, the isotope compositions of the street dust samples from Ranchito de Hu\u0026eacute;pac and Hu\u0026eacute;pac settlements, located 5 and 8 km, respectively, northeast of the tailings deposit (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e), are included along the tendency line formed by the mine tailings materials (Figs.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e and \u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e); the isotope composition supports dispersion along a northeast trend, which is the predominant wind direction (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e). In contrast, the isotope compositions of two street dust samples from Aconchi and one street dust sample from Hu\u0026eacute;pac are not aligned with the tendency line (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e), indicating the influence of additional Pb sources, for instance, from rural and municipal waste, pesticides and herbicides used in agricultural activity, leaded/unleaded gasoline (e.g., Escobar et al., \u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e2013\u003c/span\u003e; Eichler et al., \u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e2015\u003c/span\u003e; Civitillo et al., \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e2016\u003c/span\u003e; Chrastn\u0026yacute; et al., \u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e2018\u003c/span\u003e). The isotope composition of these samples exhibits a subtle inclination toward the Pb isotope compositions of Mexican gasoline (Sa\u0026ntilde;udo-Wilhemly and Flegal, 1994; Morton-Bremea et al., 2011), implying a probable influence.\u003c/p\u003e \u003cp\u003eAmong the relevant economic activities along the Sonoran River Basin, mining can contribute pollutants to the river plain. The potential contribution can be exacerbated in arid and semiarid regions, particularly during the dry seasons. If river sediments are impacted, suspension of PTE-bearing fine-grained materials can transport pollutants by wind (e.g., Moreno-Rodr\u0026iacute;guez et al., \u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e2015\u003c/span\u003e), or impacted sediments can migrate downstream. Considering the upstream spill of the Buenavista del Cobre mine in 2014, Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e shows that the Pb isotope compositions of the mine spill and impacted sediments are notably different from the studied street dust, indicating the unlikely influence of such spill over the rural dust. Regarding the Pb isotope composition of agricultural soil samples, they are included in the geogenic isotope field (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e), suggesting the close influence of the local lithology and the region's soils.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003e3.2 Pb traceability from mine tailings deposits.\u003c/h2\u003e \u003cp\u003eOne of the findings of this research highlights the importance of efflorescent salts in terms of metal traceability. Notably, the Pb isotope composition effectively constrains the signature of sulfide-rich tailings and their respective efflorescent salts. In addition, the Pb isotope composition of the efflorescent salts indicates their sensitivity to oxidation and the duration of exposure to weathering. As a result, the longer the tailings have been subjected to weathering, the more oxidized they become, leading to a Pb isotope composition similar to that of the geogenic member, as mixing with geogenic Pb is more likely under such conditions. Therefore, if efflorescent salts are formed from oxidized tailings, Pb involved in the formation of such salts will consist of a Pb mix from sulfide-rich tailings with minerals and rocks from tailings deposits, yielding isotope composition closer to the geogenic end-member (i.e., more radiogenic). In contrast, efflorescent salts formed over the sulfide-rich or slightly oxidized tailings will produce a less radiogenic composition.\u003c/p\u003e \u003cp\u003ePb traceability of efflorescent salts and oxidized mine tailings might be challenging since tailings materials are heterogeneous and geochemically complex matrices. As a consequence of the oxidation processes in arid and semi-arid environments, mine tailings can yield similar isotope composition than the geogenic end-member, which masks compositions and potentially can underestimate the influence of tailings materials over surrounding media (e.g., soils, dust, sediments). Combining mineralogical evidence, metal content, and Pb isotope composition of efflorescent salts will be crucial in accurately identifying the influence of mine tailings on environmental matrices and human health.\u003c/p\u003e \u003c/div\u003e"},{"header":"4. Conclusions","content":"\u003cp\u003eUsing the Pb isotope systematics, it is possible to identify the anthropogenic component (less radiogenic), represented by the sulfide-rich materials and respective efflorescent salts. In contrast, the Pb isotope composition of the more oxidized tailings and respective efflorescent salts is more radiogenic, trending through, and similar to the geogenic end-member. The isotope composition of street dust of the nearby settlements suggests the dispersion of the tailings materials to the surroundings. The variability of the Pb isotope composition (from less through more radiogenic) found in the efflorescent salts might be challenging when tracing pollutants in arid and semi-arid environments, especially when the geogenic member conceals the composition.\u003c/p\u003e \u003cp\u003eThe efflorescence salts in mine tailings from either historical or current mining highlight the importance of assessing the geochemical behavior to establish stabilizing procedures to avoid PTE dispersal to environmental media, considering the hazard represented by the presence of PTE hyperaccumulators and highly soluble efflorescent salts. Therefore, tracking the source, dispersion, and fate of pollutants during environmental assessments of mine-related waste from arid- and semi-arid environments is crucial. Equally important are the government's actions in establishing guidelines (e.g., characterization, mitigation, remediation, regulations) to ensure that efflorescent salts do not pose environmental and health risks. Otherwise, actions should be taken to neutralize, prevent the formation, and systematically monitor the sites of concern.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e-Funding\u003c/p\u003e\n\u003cp\u003eThis research was supported by project IN113519 (PAPIIT-UNAM), granted to Del Rio-Salas, CESUES-PTC-035 (NPCT-PRODEP), granted to Moreno-Rodr\u0026iacute;guez, and CONAHCYT-300409, granted to Loredo-Portales.\u003c/p\u003e\n\n\u003cp\u003e-\u003cstrong\u003eCompeting Interests\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eAll authors have non-financial interests to disclose.\u003c/p\u003e\n\n\u003cp\u003e-\u003cstrong\u003eConflict of interests\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eAuthors declare that they have no conflict of interest.\u003c/p\u003e\n\n\u003cp\u003e-Authors Contributions\u003c/p\u003e\n\u003cp\u003eAll authors contributed to the study conception and design and approved the final version of the manuscript.\u0026nbsp;Rafael Del Rio-Salas: conception, research design, acquisition of data, analysis, interpretation, writing original draft, review, editing. Ver\u0026oacute;nica\u003csup\u003e\u0026nbsp;\u003c/sup\u003eMoreno-Rodr\u0026iacute;guez: research design, interpretation, writing original draft, review.\u0026nbsp;Ren\u0026eacute; Loredo-Portales: analysis, interpretation, writing original draft, review.\u0026nbsp;Sergio Adri\u0026aacute;n Salgado-Souto: analysis, interpretation, writing original draft, review, editing.\u0026nbsp;Mart\u0026iacute;n Valencia-Moreno: interpretation, review, editing. Lucas Ochoa-Land\u0026iacute;n: interpretation, review, editing. Diana Romo-Morales:\u0026nbsp;acquisition of data, analysis, review, editing.\u003c/p\u003e\n\n\u003cp\u003e\u003cstrong\u003e-Ethics Approval\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eNot applicable\u003c/p\u003e\n\n\u003cp\u003e\u003cstrong\u003e-Consent to Participate\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eNot applicable\u003c/p\u003e\n\n\u003cp\u003e\u003cstrong\u003e-Consent to Publish\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eNot applicable\u003c/p\u003e\n\n\n\u003cp\u003eAcknowledgments\u003c/p\u003e\n\u003cp\u003eThis investigation was supported by project IN113519 (PAPIIT-UNAM) granted to Del Rio-Salas, CESUES-PTC-035 (NPCT-PRODEP), and CONAHCYT-300409. We thank Mark Baker for his valuable assistance during Pb isotope ratio measurements. We are thankful to J.F. Mart\u0026iacute;nez Rodr\u0026iacute;guez, A. V\u0026aacute;zquez-Salgado, L.G. Mart\u0026iacute;nez-Jardines, and D. Ramos P\u0026eacute;rez for laboratory support. We thank A. Orc\u0026iacute; Romero for preparation of mineralization samples.\u0026nbsp;We thank the CONAHCYT National Laboratories calls, the Laboratorio Nacional de Geoqu\u0026iacute;mica y Mineralog\u0026iacute;a-LANGEM, and Laboratorio de Ciencias Ambientales de la ERNO.\u003c/p\u003e\n\n"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eArchundia, D., Prado-Pano, B., Gonz\u0026aacute;lez-M\u0026eacute;ndez, B., Loredo-Portales, R., Molina-Freaner, F. (2021). Water resources affected by potentially toxic elements in an area under current and historical mining in northwestern Mexico. Environmental Monitoring and Assessment, 193(4), 1\u0026ndash;20.\u003c/li\u003e\n\u003cli\u003eCalmus, T., Valencia-Moreno, M., Del Rio-Salas, R., Ochoa-Land\u0026iacute;n, L., Mendivil-Quijada, H. (2018). A multi-elemental study to establish the natural background and geochemical anomalies in rocks from the Sonora river upper basin, NW Mexico. 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Source apportionment of heavy metals in urban road dust in a continental city of eastern China: Using Pb and Sr isotopes combined with multivariate statistical analysis. Atmospheric Environment, 201, 201\u0026ndash;211.\u003c/li\u003e\n\u003c/ol\u003e"},{"header":"Table 1","content":"\u003cp\u003eTable 1 is available in the Supplementary Files section.\u003c/p\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"environmental-geochemistry-and-health","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"egah","sideBox":"Learn more about [Environmental Geochemistry and Health](https://www.springer.com/journal/10653)","snPcode":"10653","submissionUrl":"https://submission.nature.com/new-submission/10653/3","title":"Environmental Geochemistry and Health","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Historical mine tailings, Pb isotopes, PTE dispersion, traceability, efflorescence salts","lastPublishedDoi":"10.21203/rs.3.rs-4608395/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4608395/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eDispersion of highly toxic elements associated with efflorescent crusts and mine tailings materials from historical mine sites threaten the environment and human health. Limited research has been done on traceability from historical mining sites in arid and semi-arid regions. Pb isotope systematics was applied to decipher the importance of identifying the mixing of lead sources involved in forming efflorescent salts and the repercussions on traceability. This research assessed mine waste (sulfide-rich and oxide-rich tailings material and efflorescent salts) and street dust from surrounding settlements at a historical mining site in northwestern Mexico, focusing on Pb isotope composition. The isotope data of tailings materials defined a trending line (R\u003csup\u003e2\u003c/sup\u003e\u0026thinsp;=\u0026thinsp;0.9); the sulfide-rich tailings materials and respective efflorescent salts yielded less radiogenic Pb composition, whereas the oxide-rich tailings and respective efflorescent salts yielded relatively more radiogenic compositions, similar to the geogenic component. The isotope composition of street dust suggests the dispersion of tailings materials into the surroundings. This investigation found that the variability of Pb isotope composition in tailings materials because of the geochemical heterogeneity, ranging from less radiogenic to more radiogenic, can add complexity during environmental assessments because the composition of oxidized materials and efflorescent salts can mask the geogenic component, potentially underestimating the influence on the environmental media.\u003c/p\u003e","manuscriptTitle":"Traceability and dispersion of highly toxic soluble phases from historical mine tailings","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-07-11 15:00:02","doi":"10.21203/rs.3.rs-4608395/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2024-06-24T09:42:03+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2024-06-24T09:41:39+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2024-06-20T17:37:29+00:00","index":"","fulltext":""},{"type":"submitted","content":"Environmental Geochemistry and Health","date":"2024-06-20T01:23:12+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"environmental-geochemistry-and-health","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"egah","sideBox":"Learn more about [Environmental Geochemistry and Health](https://www.springer.com/journal/10653)","snPcode":"10653","submissionUrl":"https://submission.nature.com/new-submission/10653/3","title":"Environmental Geochemistry and Health","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"2fbae938-53c8-4cb6-ad6d-916d68eb3f07","owner":[],"postedDate":"July 11th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[],"tags":[],"updatedAt":"2024-08-26T16:08:26+00:00","versionOfRecord":{"articleIdentity":"rs-4608395","link":"https://doi.org/10.1007/s10653-024-02180-3","journal":{"identity":"environmental-geochemistry-and-health","isVorOnly":false,"title":"Environmental Geochemistry and Health"},"publishedOn":"2024-08-24 15:57:21","publishedOnDateReadable":"August 24th, 2024"},"versionCreatedAt":"2024-07-11 15:00:02","video":"","vorDoi":"10.1007/s10653-024-02180-3","vorDoiUrl":"https://doi.org/10.1007/s10653-024-02180-3","workflowStages":[]},"version":"v1","identity":"rs-4608395","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4608395","identity":"rs-4608395","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}